From Ion Current to Electroosmotic Flow Rectification in Asymmetric Nanopore Membranes.
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ABSTRACT:
SUBMITTER: Experton J
PROVIDER: S-EPMC5746935 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Ion current rectification (ICR) is a transport phenomenon in which an electrolyte conducts unequal currents at equal and opposite voltages. Here, we show that nanoscale fluid vortices and nonlinear electroosmotic flow (EOF) drive ICR in the presence of concentration gradients. The same EOF can yield negative differential resistance (NDR), in which current decreases with increasing voltage. A finite element model quantitatively reproduces experimental ICR and NDR recorded across glass nanopipettes under concentration gradients. The model demonstrates that spatial variations of electrical double layer properties induce the nanoscale vortices and nonlinear EOF. Experiments are performed in conditions directly related to scanning probe imaging and show that quantitative understanding of nanoscale transport under concentration gradients requires accounting for EOF. This characterization of nanopipette transport physics will benefit diverse experimentation, pushing the resolution limits of chemical and biophysical recordings.
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Project description:Unveiling the contributions of electroosmotic flow (EOF) in the electrokinetic transport through structurally-defined nanoscale pores and channels is challenging but fundamentally significant because of the broad relevance of charge transport in energy conversion, desalination and analyte mixing, micro and nano-fluidics, single entity analysis, capillary electrophoresis etc. This report establishes a universal method to diagnose and deconvolute EOF in the nanoscale transport processes through current-potential measurements and analysis without simulation. By solving Poisson, Nernst-Planck (PNP) with and without Navier-Stokes (NS) equations, the impacts of EOF on the time-dependent ion transport through asymmetric nanopores are unequivocally revealed. A sigmoidal shape in the I-V curves indicate the EOF impacts which further deviate from the well-known non-linear rectified transport features. Two conductance signatures, an absolute change in conductance and a 'normalized' one relative to ion migration, are proposed as EOF impact (factor). The EOF impacts can be directly elucidated from current-potential experimental results from the two analytical parameters without simulation. The EOF impact is found more significant in intermediate ionic strength, and potential and pore size dependent. The less-intuitive ionic strength and size dependence is explained by the combined effects of electrostatic screening and non-homogeneous charge distribution/transport at nanoscale interface. The time-dependent conductivity and optical imaging experiments using single nanopipettes validate the proposed method which is applicable to other channel type nanodevices and membranes. The generalizable approach eliminates the need of simulation/fitting of specific experiments and offers previously inaccessible insights into the nanoscale EOF impacts under various experimental conditions for the improvement of separation, energy conversions, high spatial and temporal control in single entity sensing/manipulation, and other related applications.
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Project description:The ionic current rectification (ICR) is a non-linear current-voltage response upon switching the polarity of the potential across nanopore which is similar to the I-V response in the semiconductor diode. The ICR phenomenon finds several potential applications in micro/nano-fluidics (e.g., Bio-sensors and Lab-on-Chip applications). From a biological application viewpoint, most biological fluids (e.g., blood, saliva, mucus, etc.) exhibit non-Newtonian visco-elastic behavior; their rheological properties differ from Newtonian fluids. Therefore, the resultant flow-field should show an additional dependence on the rheological material properties of viscoelastic fluids such as fluid relaxation time [Formula: see text] and fluid extensibility [Formula: see text]. Despite numerous potential applications, the comprehensive investigation of the viscoelastic behavior of the fluid on ionic concentration profile and ICR phenomena has not been attempted. ICR phenomena occur when the length scale and Debye layer thickness approaches to the same order. Therefore, this work extensively investigates the effect of visco-elasticity on the flow and ionic mass transfer along with the ICR phenomena in a single conical nanopore. The Poisson-Nernst-Planck (P-N-P) model coupled with momentum equations have been solved for a wide range of conditions such as, Deborah number, [Formula: see text], Debye length parameter, [Formula: see text], fluid extensibility parameter, [Formula: see text], applied electric potential, [Formula: see text], and surface charge density [Formula: see text] and [Formula: see text]. Limited results for Newtonian fluid ([Formula: see text], and [Formula: see text]) have also been shown in order to demonstrate the effectiveness of non-Newtonian fluid behaviour over the Newtonian fluid behaviour. Four distinct novel characteristics of electro-osmotic flow (EOF) in a conical nanopore have been investigated here, namely (1) detailed structure of flow field and velocity distribution in viscoelastic fluids (2) influence of Deborah number and fluid extensibility parameter on ionic current rectification (ICR) (3) volumetric flow rate calculation as a function of Deborah number and fluid extensibility parameter (4) effect of viscoelastic parameters on concentration distribution of ions in the nanopore. At high applied voltage, both the extensibility parameter and Deborah number facilitate the ICR phenomena. In addition, the ICR phenomena are observed to be more pronounced at low values of [Formula: see text] than the high values of [Formula: see text]. This effect is due to the overlapping of the electric double layer at low values of [Formula: see text].
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Project description:Ion current rectification (ICR), defined as an increase in ion conduction at a given polarity and a decrease in ion conduction for the same voltage at the opposite polarity, i.e., a deviation from a linear ohmic response, occurs in conical shaped pores due to the voltage dependent solution conductivity within the aperture. The degree to which the ionic current rectifies is a function of the size and surface charge of the nanopore, with smaller and more highly charged pores exhibiting greater degrees of rectification. The ICR phenomenon has previously been exploited for biosensing applications, where the level of ICR for a nanopore functionalized with an analyte-specific binding molecule (e.g., an antibody, biotin, etc.) changes upon binding its target analyte (e.g., an antigen, streptavidin, etc.) due to a resulting change in the size and/or charge of the aperture. While this type of detection measurement is typically qualitative, for the first time, we demonstrate that the rate at which the nanopore ICR response changes is dependent on the concentration of the target analyte introduced. Utilizing a glass nanopore membrane (GNM) internally coated with a monoclonal antibody specific to the cleaved form of synaptosomal-associated protein 25 (cSNAP-25), creating the antibody-modified glass nanopore membrane (AMGNM), we demonstrate a correlation between the rate of ICR change and the concentration of introduced cSNAP-25, over a range of 500 nM-100 ?M. The methodology presented here significantly expands the applications of nanopore ICR biosensing measurements and demonstrates that these measurements can be quantitative in nature.
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Project description:We describe ion distribution and the current-voltage (i-V) response of nanopipettes at different probe-to-substrate distances (Dps) as simulated by finite-element methods. Results suggest electrostatic interactions between a charged substrate and the nanopipette dominate electrophoretic ion transport through the nanopipette when Dps is within 1 order of magnitude of the Debye length (∼10 nm for a 1 mM solution as employed in the simulation). Ion current rectification (ICR) and permselectivity associated with a neutral or charged nanopipette can be reversibly enhanced or reduced dependent on Dps, charge polarity, and charge density (σ) of the substrate. Regulation of nanopipette current is a consequence of the enrichment or depletion of ions within the nanopipette interior, which influences conductivity of the nanopipette. When the external substrate is less negatively charged than the nanopipette, the substrate first reduces, and then enhances the ICR as Dps decreases. Surprisingly, both experimental and simulated data show that a neutral substrate was also able to reduce and reverse the ICR of a slightly negatively charged nanopipette. Simulated results ascribe such effects to the elimination of ion depletion within the nanopipette at positive potentials.
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